Method of improving electrode-to-solid-electrolyte interface contact in solid-state batteries

Abstract

A method of improving interfacial contact at an electrode-to-solid-electrolyte interface in a solid-state battery cell is provided. The method includes providing a solid-state battery cell including a solid-state electrolyte and electrodes defining an anode and a cathode. Each of the anode and cathode are adjacent to the solid-state electrolyte at an interface. The method further includes electrochemically increasing interfacial contact between at least one of the electrodes and the solid-state electrolyte by applying a voltage pulse to the cell at a high current density for a short duration, wherein electrode material diffuses into pores formed in the solid electrolyte interface, thereby healing the pores and eliminating an interfacial space charge effect.

What is claimed is: 
     
         1 . A method of improving interfacial contact at an electrode-to-solid-electrolyte interface in a solid-state battery cell, the method comprising:
 providing a solid-state battery cell including a solid-state electrolyte and electrodes defining an anode and a cathode, wherein each of the anode and cathode are adjacent to the solid-state electrolyte at an interface;   electrochemically increasing interfacial contact between at least one of the electrodes and the solid-state electrolyte by applying a voltage pulse to the cell at a high current density for a short duration, wherein electrode material diffuses into pores formed in the solid electrolyte interface, thereby healing the pores and eliminating an interfacial space charge effect.   
     
     
         2 . The method of  claim 1 , wherein the voltage pulse has a cut-off voltage having an absolute value greater than or equal to 20 V at a cell level. 
     
     
         3 . The method of  claim 2 , wherein the cut-off voltage of the voltage pulse has an absolute value greater than or equal to 10 V at a cell level. 
     
     
         4 . The method of  claim 1 , wherein the high current density applied to the cell is at least five times greater than the critical current density at a cell level. 
     
     
         5 . The method of  claim 1 , wherein the high current density applied to the cell is greater than or equal to 10 mA cm -2  at a cell level. 
     
     
         6 . The method of  claim 1 , wherein the short duration is greater than or equal to 0.1 ms. 
     
     
         7 . The method of  claim 6 , wherein the short duration is in a range of 0.1 to 0.5 ms. 
     
     
         8 . The method of  claim 1 , wherein the short duration is less than 1 ms. 
     
     
         9 . The method of  claim 1 , wherein the voltage pulse includes more than one pulse cycle. 
     
     
         10 . The method of  claim 1 , wherein the solid-state electrolyte is one of an inorganic solid electrolyte, a solid polymer electrolyte, and a composite polymer electrolyte. 
     
     
         11 . The method of  claim 10 , wherein the solid-state electrolyte is one of a garnet, a NASICON, a LISICON, an argyrodite-like, a lithium nitride, a lithium hydride, a lithium halide, a lithium phosphorous oxynitride, a lithium thiophosphate, a perovskite, a polyether-based electrolyte, a polycarbonate-based electrolyte, a polyester-based electrolyte, a polynitrile-based electrolyte, a polyalcohol-based electrolyte, a polyamine-based electrolyte, a polysiloxane-based electrolyte, a fluoropolymer-based electrolyte, a gel polymer electrolyte, an ionogel electrolyte, and a gel electrolyte. 
     
     
         12 . The method of  claim 1 , wherein the anode comprises a Li-based active material, a Na-based active material, a K-based active material, a Mg-based active material, or a Zn-based active material. 
     
     
         13 . The method of  claim 1 , wherein the pores in the solid-state electrolyte are reduced or completely filled up due to local heating of the anode material at the interface in the vicinity of the pores. 
     
     
         14 . The method of  claim 1 , wherein the method is performed in-operando. 
     
     
         15 . A solid-state battery cell having an electrochemical performance improved by the method of  claim 1 .